Dataset Information

Stable Hexylphosphonate-Capped Blue-Emitting Quantum-Confined CsPbBr₃ Nanoplatelets.

ABSTRACT: Quantum-confined CsPbBr₃ nanoplatelets (NPLs) are extremely promising for use in low-cost blue light-emitting diodes, but their tendency to coalesce in both solution and film form, particularly under operating device conditions with injected charge-carriers, is hindering their adoption. We show that employing a short hexyl-phosphonate ligand (C₆H₁₅O₃P) in a heat-up colloidal approach for pure, blue-emitting quantum-confined CsPbBr₃ NPLs significantly suppresses these coalescence phenomena compared to particles capped with the typical oleyammonium ligands. The phosphonate-passivated NPL thin films exhibit photoluminescence quantum yields of ?40% at 450 nm with exceptional ambient and thermal stability. The color purity is preserved even under continuous photoexcitation of carriers equivalent to LED current densities of ?3.5 A/cm². ¹³C, ¹³³Cs, and ³¹P solid-state MAS NMR reveal the presence of phosphonate on the surface. Density functional theory calculations suggest that the enhanced stability is due to the stronger binding affinity of the phosphonate ligand compared to the ammonium ligand.

SUBMITTER: Shamsi J

PROVIDER: S-EPMC7296617 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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Publications

Stable Hexylphosphonate-Capped Blue-Emitting Quantum-Confined CsPbBr3 Nanoplatelets.

Shamsi Javad J Kubicki Dominik D Anaya Miguel M Liu Yun Y Ji Kangyu K Frohna Kyle K Grey Clare P CP Friend Richard H RH Stranks Samuel D SD

ACS energy letters 20200515 6

Quantum-confined CsPbBr3 nanoplatelets (NPLs) are extremely promising for use in low-cost blue light-emitting diodes, but their tendency to coalesce in both solution and film form, particularly under operating device conditions with injected charge-carriers, is hindering their adoption. We show that employing a short hexyl-phosphonate ligand (C6H15O3P) in a heat-up colloidal approach for pure, blue-emitting quantum-confined CsPbBr3 NPLs sign ...[more]

PMID: 32566752

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Project description:Ligand-capped nanocrystals (NCs) of lead halide perovskites, foremost fully inorganic CsPbX3 NCs, are the latest generation of colloidal semiconductor quantum dots. They offer a set of compelling characteristics-large absorption cross section, as well as narrow, fast, and efficient photoluminescence with long exciton coherence times-rendering them attractive for applications in light-emitting devices and quantum optics. Monodisperse and shape-uniform, broadly size-tunable, scalable, and robust NC samples are paramount for unveiling their basic photophysics, as well as for putting them into use. Thus far, no synthesis method fulfilling all these requirements has been reported. For instance, long-chain zwitterionic ligands impart the most durable surface coating, but at the expense of reduced size uniformity of the as-synthesized colloid. In this work, we demonstrate that size-selective precipitation of CsPbBr3 NCs coated with a long-chain sulfobetaine ligand, namely, 3-(N,N-dimethyloctadecylammonio)-propanesulfonate, yields monodisperse and sizable fractions (>100 mg inorganic mass) with the mean NC size adjustable in the range between 3.5 and 16 nm and emission peak wavelength between 479 and 518 nm. We find that all NCs exhibit an oblate cuboidal shape with the aspect ratio of 1.2 × 1.2 × 1. We present a theoretical model (effective mass/k·p) that accounts for the anisotropic NC shape and describes the size dependence of the first and second excitonic transition in absorption spectra and explains room-temperature exciton lifetimes. We also show that uniform zwitterion-capped NCs readily form long-range ordered superlattices upon solvent evaporation. In comparison to more conventional ligand systems (oleic acid and oleylamine), supercrystals of zwitterion-capped NCs exhibit larger domain sizes and lower mosaicity. Both kinds of supercrystals exhibit superfluorescence at cryogenic temperatures-accelerated collective emission arising from the coherent coupling of the emitting dipoles.

Dataset Information

Stable Hexylphosphonate-Capped Blue-Emitting Quantum-Confined CsPbBr₃ Nanoplatelets.

Publications

Stable Hexylphosphonate-Capped Blue-Emitting Quantum-Confined CsPbBr<sub>3</sub> Nanoplatelets.

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